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Cellulose-<i>grafte</i>-poly(L-lactide) (C-<i>g</i>-PLLA) copolymers synthesized in a CO₂-switchable solvent are proposed for use as effective compatibilizers for the preparation of cellulose–PLLA composites with enhanced interfacial compatibility. The effect of the molar substitution (<i>MS</i>_PLLA) of the grafted PLLA side chain in the C-<i>g</i>-PLLA copolymer and the feeding amount of this copolymer on the mechanical and thermal properties and hydrophilicity of the composites was investigated. The composites had a largely increased impact strength with the incorporation of the compatibilizer. With the increasing of <i>MS</i>_PLLA and the feeding amount of the copolymer, the resulting composites had an increased impact strength. When 5 wt% C-<i>g</i>-PLLA with <i>MS</i>_PLLA of 4.46 was used as a compatibilizer, the obtained composite containing 20 wt% cellulose presented an impact strength equal to that obtained for the neat PLLA. The composites had a slightly decreased melting temperature and thermal decomposition temperature, but increased hydrophilicity due to the incorporation of the compatibilizer. This work suggests an effective method to improve the interfacial compatibility between cellulose and PLLA for the fabrication of fully bio-based composites with high performance.